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Adsorption of methane, ethane and ethylene on molecular sieve zeolites 分子筛分子筛对甲烷、乙烷和乙烯的吸附
Pub Date : 1996-01-01 DOI: 10.1016/0950-4214(95)00016-X
R.W. Triebe, F.H. Tezel, K.C. Khulbe

Adsorption of pure methane, ethane and ethylene on molecular sieve zeolites was examined via the gas chromatographic method to determine the potential for the separation of ethylene from light hydrocarbons. The molecular sieves chosen for the study were H-mordenite and 13X, CaX, 4A and 5A zeolites. Henry's law constants were determined over a variety of temperature ranges between 233 and 473 K. van't Hoff plots are presented for all three gases on 4A and 5A zeolites and for methane and ethylene on the CaX and 13X zeolites and H-mordenite. Equilibrium separation factors for the ethylene/methane system are provided for all zeolites (except clinoptilolite) over various temperature ranges. Separation is most promising with CaX zeolite, which yielded separation factors ranging from 1100 at 100 °C to 100 at 200 °C. Separation seems possible in 5A and CaX zeolites at very high temperatures due to the strong affinity of their divalent cations for the ethylene π-bond.

采用气相色谱法研究了分子筛分子筛对纯甲烷、乙烷和乙烯的吸附,以确定乙烯从轻烃中分离的潜力。选用的分子筛为h -丝光沸石和13X、CaX、4A和5A沸石。在233 - 473 k的不同温度范围内测定了亨利定律常数,给出了4A和5A沸石上所有三种气体的范霍夫图,以及CaX和13X沸石和h -丝光沸石上甲烷和乙烯的范霍夫图。所有沸石(斜沸石除外)在不同温度范围内提供了乙烯/甲烷体系的平衡分离因子。用CaX沸石进行分离是最有希望的,在100°C时得到的分离因子为1100,在200°C时为100。在5A和CaX分子筛中,由于它们的二价阳离子对乙烯π键有很强的亲和力,在非常高的温度下分离似乎是可能的。
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引用次数: 102
Equilibrium concentration profiles of species in CO2—alkanolamine—water systems 二氧化碳-烷醇胺-水体系中物种平衡浓度分布
Pub Date : 1996-01-01 DOI: 10.1016/0950-4214(95)00021-6
M.Z. Haji-Sulaiman, M.K. Aroua, Md Ilyas Pervez

Equilibrium concentrations of species and gas loading in aqueous solutions of alkanolamine loaded with CO2 are being compared with predicted profiles obtained from the Deshmukh-Mather Model. A new technique is being proposed based on titration using a base, NaOH, to determine the concentrations of the different species at equilibrium. The technique is reliable and easy to perform to give reproducible results. Experimental and predicted concentrations of species are in good agreement over a range of gas loading between 0.4 and 1.0 for aqueous AMP solutions. For DEA, the predicted and measured values complement each other at high loading typically above 0.6. At low loading, there is a significant difference between the sets of values for carbamate and bicarbonate. These differences are likely due to the value of the equilibrium constant for the carbamate formation, which is taken as an adjustable parameter in the model, to give the best fit to the experimental data of either CO2 partial pressure or gas loading.

将载有二氧化碳的烷醇胺水溶液中物种平衡浓度和气体负荷与从Deshmukh-Mather模型获得的预测剖面进行了比较。有人提出了一种新的技术,基于滴定使用碱,氢氧化钠,以确定在平衡状态下不同物种的浓度。该技术可靠,易于操作,结果可重复性好。实验和预测的物质浓度在0.4和1.0的气体负载范围内是一致的。对于DEA,在高负荷时,预测值和实测值通常大于0.6。在低负荷下,氨基甲酸酯和碳酸氢盐的值组之间存在显著差异。这些差异可能是由于氨基甲酸酯形成的平衡常数的值,这是一个可调的参数,在模型中,给出了最佳拟合的实验数据,无论是CO2分压或气体负荷。
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引用次数: 32
Measurement and analysis of oxygen/nitrogen/ 5A-zeolite adsorption equilibria for air separation 空气分离中氧/氮/ 5a -沸石吸附平衡的测定与分析
Pub Date : 1996-01-01 DOI: 10.1016/0950-4214(96)00014-X
Orhan Talu , Jianmin Li , Ravi Kumar , Paul M. Mathias , J.Douglas Moyer Jr , Joan M. Schork

Multicomponent adsorption equilibrium data are essential for the reliable design of processes and equipment for gas separation by adsorption. We discuss techniques for the measurement and analysis of multicomponent adsorption equilibrium data, and present a comprehensive set of equilibrium data for the adsorption of oxygen and nitrogen on 5A-zeolite.

多组分吸附平衡数据对于气体吸附分离工艺和设备的可靠设计至关重要。我们讨论了多组分吸附平衡数据的测量和分析技术,并提出了一套完整的氧和氮在5a -沸石上吸附的平衡数据。
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引用次数: 48
A study on catalytic membrane reactors for water gas shift reaction 水煤气移位反应催化膜反应器的研究
Pub Date : 1996-01-01 DOI: 10.1016/0950-4214(95)00023-2
A. Basile , E. Drioli , F. Santell , V. Violante , G. Capannelli , G. Vitulli

In the present work the water gas shift reaction is considered as a particular application of a catalytic membrane reactor. Three different methods to deposit a thin film of palladium on a porous ceramic tubular membrane have been studied: the magnetron sputtering technique, the physical vapour deposition technique, and the co-condensation technique or solvated metal atom deposition method. For each composite membrane, characterization in terms of pore distribution, thickness of the film, percentage of Pd deposited along the thickness of the membrane and CO conversion versus feed flow rate and versus different H2OCO molar ratio are presented.

本文将水煤气移位反应作为催化膜反应器的一种特殊应用。研究了在多孔陶瓷管膜上沉积钯薄膜的三种不同方法:磁控溅射技术、物理气相沉积技术和共冷凝技术或溶剂化金属原子沉积方法。对每一种复合膜,从孔分布、膜厚度、沿膜厚度沉积的Pd百分比、CO转化率随进料流量和不同H2OCO摩尔比的变化等方面进行了表征。
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引用次数: 82
Modelling endothermic reactions in a compound membrane reactor 模拟复合膜反应器中的吸热反应
Pub Date : 1996-01-01 DOI: 10.1016/0950-4214(95)00018-6
S. Assabumrungrat, D.A. White

This paper models the performance of a membrane reactor. The membrane, a composite alumina-based one, is packed with a catalyst and allows low molecular weight gases to diffuse through it at a faster rate than gases with a higher molecular weight. This allows a greater conversion to be achieved in one pass through the reactor. The reaction that is specifically considered in this paper is the dehydrogenation of methyl-cyclohexane to toluene with the production of hydrogen. This latter species is preferentially removed by the membrane. Data for the performance of the membrane have been estimated from previous experiments using single gases and the mechanisms considered are Knudsen and bulk flow. Surface flow is not considered in the model as it is possibly not important as the endothermic reaction is carried out at a high temperature. A standard kinetic model is also incorporated in the calculations. The correlations of maximum effective length of membrane reactors and maximum percentage conversion as functions of the feed velocity and the membrane diameter are demonstrated in this paper. This paper also considers the behaviour of a compound reactor in which the first section is a straightforward ‘plug flow’ reactor where the catalyst is confined in an impermeable tube with the same internal diameter as the membrane. This is followed by a section containing the membrane. The reason for considering this configuration is to avoid unnecessary leakage of methyl-cyclohexane feed in the initial stages of the reaction. This innovation leads to predicted increases in the overall conversion of the process.

本文对膜反应器的性能进行了模拟。这种膜是一种基于氧化铝的复合膜,它被催化剂包裹,使低分子量气体比高分子量气体以更快的速度扩散。这允许在一次通过反应器时实现更大的转化。本文具体考虑的反应是甲基环己烷脱氢制甲苯产氢。后一种被膜优先去除。膜性能的数据已经从以前使用单一气体的实验中估计出来,所考虑的机制是克努森和体流。模型中没有考虑表面流动,因为吸热反应在高温下进行,表面流动可能不重要。在计算中还采用了标准动力学模型。本文论证了膜反应器最大有效长度和最大转化率随进料速度和膜直径的关系。本文还考虑了复合反应器的行为,其中第一部分是直接的“塞流”反应器,其中催化剂被限制在具有与膜相同内径的不透水管中。接下来是一个包含膜的部分。考虑这种配置的原因是为了避免在反应的初始阶段出现不必要的甲基环己烷进料泄漏。这种创新导致了整个过程的预期转换的增加。
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引用次数: 2
UNIFAC activity coefficient derivatives UNIFAC活度系数导数
Pub Date : 1996-01-01 DOI: 10.1016/0950-4214(96)00018-7
P. Pöllmann , M. Löbbecke

A scheme is presented for the calculation of the UNIFAC activity coefficient and its analytical derivatives with respect to mole fractions and with respect to temperature. A numerical example is also given.

提出了一种计算UNIFAC活度系数及其对摩尔分数和温度的解析导数的方法。并给出了数值算例。
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引用次数: 1
Performance of a hollow fibre membrane unit in oxygen-enriched air production 中空纤维膜装置在富氧空气生产中的性能
Pub Date : 1996-01-01 DOI: 10.1016/0950-4214(96)00012-6
Claudio Fabiani , Luigi Bimbi , Massimo Pizzichini , Luigi Santarossa

The performance of a pilot test for biogas upgrading has been tested under different process conditions to produce oxygen-enriched air for aqueous media application. The selectivity of the polysulfone hollow fibres for N2O2 permeation allows the production of an oxygen-enriched air stream in the 30–50% range and an inert gas (nitrogen between 82–98%) by operating the pilot unit at different stage-cut values in a single pass mode. Membrane area requirements for a medium size plant of 100 Nm3 h−1 are discussed according to a simple perfect mixing model for gas permeation.

在不同的工艺条件下进行了沼气升级中试的性能测试,以生产用于水介质的富氧空气。聚砜中空纤维对N2O2渗透的选择性允许通过在单道模式下以不同的阶段切割值操作中试装置,产生30-50%范围内的富氧气流和惰性气体(氮气在82-98%之间)。根据气体渗透的简单完美混合模型,讨论了100 Nm3 h−1中型装置对膜面积的要求。
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引用次数: 8
Modeling of gas absorption into turbulent films with chemical reaction 用化学反应模拟湍流膜中的气体吸收
Pub Date : 1996-01-01 DOI: 10.1016/0950-4214(95)00024-0
Mohammad R. Riazi

A mathematical model has been developed to predict the rates of gas absorption in turbulent falling liquid films with and without the first order homogeneous reaction and external gas phase mass transfer resistance. The eddy viscosity model used to describe the flow distribution is the van Driest model, modified in the outer region of the film by the use of an eddy diffusivity deduced from gas absorption measurements. The results are given for special cases to illustrate the effects of turbulence, reaction rate and gas phase resistances on the concentration profiles and the rates of gas absorption.

建立了一个数学模型,用于预测有或没有一级均相反应和外部气相传质阻力时湍流下降液膜中的气体吸收率。用于描述流动分布的涡流粘度模型是van Driest模型,该模型在膜的外部区域通过使用从气体吸收测量中推导出的涡流扩散系数进行了修正。给出了特殊情况下的结果,以说明湍流、反应速率和气相阻力对浓度分布和气体吸收速率的影响。
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引用次数: 5
Gas solubility maxima in mixtures of physical absorbents and chemisorbents 在物理吸收剂和化学吸收剂的混合物中气体溶解度最大
Pub Date : 1996-01-01 DOI: 10.1016/0950-4214(95)00029-1
I.L. Leites , J.G. Karpova, V.M. Berchenko

Experimental data demonstrate that mixing of absorbents gives the possibility to increase gas solubility. This effect may be predicted using a simplified theory of solution. Solution theory predicts that increasing solubility is possible in mixtures with positive deviations from Raul's law and when some other conditions exist. This effect is greatest near lamination of solvent mixture. Gas solubility in regular solution may increase not more than 1.6 times. A similar effect may arise when mixing chemisorbents. This effect is very large. When an equal saturation degree of solution by gas is fixed, the equilibrium pressure of gas above solution may decrease by 10–50 times as compared with the pressure above the solution of one of the chemisorbents. Theory and experiment demonstrate that the positive effect is greatest when the saturation degree is small, and this effect becomes negative when the saturation degree is great. These results give a new explanation for the effect of chemisorbent mixing in industrial processes such as the Benfield process.

实验数据表明,混合吸收剂有可能增加气体溶解度。这种效应可以用一种简化的解理论来预测。溶液理论预测,在偏离劳尔定律的混合物中,当存在一些其他条件时,溶解度的增加是可能的。这种效应在溶剂混合物层压时最为明显。气体在常规溶液中的溶解度可增加不超过1.6倍。在混合化学助剂时也会产生类似的效果。这种影响非常大。当气体溶液的饱和度相等时,溶液上气体的平衡压力可能比其中一种化学同色剂溶液的平衡压力降低10-50倍。理论和实验表明,当饱和度较小时,正效应最大,当饱和度较大时,正效应变为负效应。这些结果为化学吸附剂混合在工业过程(如本菲尔德过程)中的作用提供了新的解释。
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引用次数: 0
Extension of the linear driving force-dusty gas model approximation to include surface or micropore diffusion 线性驱动力-含尘气体模型近似的扩展,以包括表面或微孔扩散
Pub Date : 1996-01-01 DOI: 10.1016/0950-4214(96)00013-8
Adélio M.M. Mendes, Carlos A.V. Costa, Alírio E. Rodrigues

This paper presents linear driving force approximations for the dusty gas model in a bisolute system obeying linear or Langmuir isotherms, in two situations: when there is a nonnegligible surface flux in parallel with the diffusive and convective fluxes; and when there is a micropore resistance to mass transfer in series. The approximations were developed using a semi-empirical procedure that starts with the particle response to a square wave perturbation considering a simple diffusion/convection mechanism, and proceeds by consecutive corrections to this basic result. These corrections are obtained using superposition, similarity and pattern recognition. The approximations are good (average quadratic error ⩽10%) when representing the system cyclic steady state, whether the perturbations are sharp or smooth.

本文给出了服从线性等温线或Langmuir等温线的绝对系统中含尘气体模型在两种情况下的线性驱动力近似:当存在不可忽略的表面通量与扩散通量和对流通量平行时;当存在微孔时,传质阻力串联。近似是使用半经验程序开发的,该程序从考虑简单扩散/对流机制的粒子对方波扰动的响应开始,然后通过连续修正该基本结果。这些校正是通过叠加、相似度和模式识别得到的。当表示系统循环稳态时,无论扰动是剧烈的还是平滑的,近似都很好(平均二次误差≤10%)。
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引用次数: 8
期刊
Gas Separation & Purification
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